Date of Award

10-14-2024

Author's School

Graduate School of Arts and Sciences

Author's Department

Chemistry

Degree Name

Doctor of Philosophy (PhD)

Degree Type

Dissertation

Abstract

Antimicrobial resistance is a growing global health crisis, with enzymatic inactivation being particularly concerning, as it can diminish the efficacy of antibiotics across an entire infection environment. This dissertation focuses on tetracycline antibiotics and the emerging class of tetracycline destructases (TDases), which are following a similar evolutionary path as beta-lactamase enzymes. Our research explored various strategies to counteract this resistance, including the design and evaluation of TDase inhibitors derived from anhydrotetracycline. We developed two series of inhibitors: C9-anhydrotetracycline derivatives, which effectively block both tetracycline and NADPH binding, and C10-anhydrotetracyclne derivatives, which improved water solubility and whole-cell activity against multiple bacterial species. Additionally, we pioneered a new approach to combat antibiotic enzymatic inactivation using targeted protein degradation of TetX in Mycobacteria. Through comprehensive analysis of TDase activity, structure, inhibition, and degradation, this work provides a framework for restoring the potency of tetracyclines against resistant bacterial strains.

Language

English (en)

Chair and Committee

Timothy Wencewicz

Committee Members

Christina Stallings; Gautam Dantas; John-Stephen Taylor; Kevin Moeller

Available for download on Friday, December 21, 2029

Included in

Chemistry Commons

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